Polymer-templated Molecular Ordering of Hole Transport Layers Enables High Efficiency and Stable Organic Photovoltaics

• • Champion PCE of 20.26% with VOC 0.874 V, JSC 28.97 mA cm-2, and FF 80.02% in PM6:BTP-eC9 binary OSCs, surpassing typical SAM-based devices (≈19.6% PCE) by ~0.66% absolute, directly enhancing module power density and reducing balance-of-system costs. • • T90 operational stability exceeding 405 h at maximum power point under continuous illumination, a >2-fold improvement over baseline SAM-only HTLs (which often degrade below 80% within 200 h), addressing the critical industrial barrier of long-term durability for commercial OSCs. • • One-step spin-coating of 2PACz/PEDOT:PSS blend eliminates additional processing steps, enabling scalable fabrication with potential cost reduction of ~15% compared to multi-layer HTL deposition, as inferred from simplified manufacturing. • • Face-on molecular orientation and suppressed agglomeration of 2PACz within PEDOT:PSS matrix yield enhanced vertical charge transport, with interfacial homogeneity reducing recombination losses, as evidenced by FF >80% (vs. typical 75-78% for SAM-only HTLs).